In this study, the structure, electrical and thermal properties of ten polymer compositions based on polylactic acid (PLA), low-cost industrial graphene nanoplates (GNP) and multi-walled carbon nanotubes (MWCNT) in mono-filler PLA/MWCNT and PLA/GNP systems with 0–6 wt.% filler content were investigated. Filler dispersion was further improved by combining these two carbon nanofillers with different geometric shapes and aspect ratios in hybrid bi-filler nanocomposites. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and Raman spectroscopy exhibited uniform dispersion of nanoparticles in a polymer matrix. The obtained results have shown that for the mono-filler systems with MWCNT or GNP, the electrical conductivity increased with decades. Moreover, a small synergistic effect was observed in the GNP/MWCNT/PLA bi-filler hybrid composites when combining GNP and CNT at a ratio of 3% GNP/3% CNT and 1.5% GNP:4.5% CNT, showing higher electrical conductivity with respect to the systems incorporating individual CNTs and GNPs at the same overall filler concentration. This improvement was attributed to the interaction between CNTs and GNPs limiting GNP aggregation and bridging adjacent graphene platelets thus, forming a more efficient network. Thermal conductivity increases with higher filler content; this effect was more pronounced for the mono-filler composites based on PLA and GNP due to the ability of graphene to better transfer the heat. Morphological analysis carried out by electron microscopy (SEM, TEM) and Raman indicated that the nanocomposites present smaller and more homogeneous filler aggregates. The well-dispersed nanofillers also lead to a microstructure which is able to better enhance the electron and heat transfer and maximize the electrical and thermal properties. The obtained composites are suitable for the production of a multifunctional filament with improved electrical and thermal properties for different fused deposition modelling (FDM) 3D printing applications and also present a low production cost, which could potentially increase the competitiveness of this promising market niche.
The reinforcing effect of carbon nanoparticles in an epoxy resin has been estimated with different approaches based on rheology, molecular dynamics (evaluated by differential scanning calorimetry, dielectric relaxation spectroscopy, and thermally stimulated depolarization current), and dynamic mechanical analysis. Carbon particles aggregate as the volume increases and form a fractal structure in the matrix polymer. The dispersion microstructure has been characterized by its viscoelastic properties and relaxation time spectrum. The scaling of the storage modulus and yield stress with the volume fraction of carbon shows two distinct exponents and has thus been used to determine the critical carbon volume fraction of the network formation (Φ*) for the carbon/epoxy dispersions. At nanofiller concentrations greater than Φ*, the overall mobility of the polymer chains is restricted in both dispersions and solid nanocomposites. Therefore, (1) the relaxation spectrum of the dispersions is strongly shifted toward longer times, (2) the glass‐transition temperature is increased and (3) the relaxation strength of both the secondary (β) and primary (α) relaxations increases in the nanocomposites, with respect to the pure polymer matrix. The dispersion microstructure, consisting of fractal flocs and formed above Φ*, is proposed to play the main role in the reinforcement of nanocomposites. Moreover, the network structure and the interface polymer layer (bond layer), surrounding nanoparticles, increases the relaxation strength and slows the cooperative α relaxation, and this results in an improvement of the mechanical properties. © 2005 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 43: 522–533, 2005
Electromagnetic and thermal properties of a non-conventional polymer nanocomposite based on thermoplastic Polylactic acid (PLA, Ingeo™) filled, in different weight percentage, with multi-walled carbon nanotubes (MWCNTs), graphene nanoplatelets (GNPs), as well as a mixture of both fillers (MWCNTs/GNPs), are analyzed. The combination of notable electrical, thermal, and electromagnetic (EM) properties of the carbon fillers, in concentrations above the percolation threshold, together with the good processability of the PLA matrix gives rise to innovative filaments for 3D printing. In particular, the shielding efficiency (SE) in the frequency range 26–37 GHz of samples increases from 0.20 dB of unfilled PLA up to 13.4 dB for composites containing MWCNTs and GNPs, corresponding to 4% and 95% of SE, respectively. The thermal conductivity of the PLA loaded with 12 wt % of GNPs is 263% higher than that of the unfilled polymer, whereas an improvement of about 99% and 190% is detected for the PLA matrix loaded with MWCNTs and both fillers, respectively. The EM and thermal characterization is combined with a morphological investigation allowing us to correlate the dispersion states of the fillers within the polymer matrix with the observed EM and thermal properties. The EM and thermal characteristics exhibited by the nanocomposites make them suitable for packaging applications of electronic devices with electromagnetic interference (EMI) shielding and thermal dissipation features.
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